Line shape of time-resolved four-wave mixing

Time-resolved four-wave-mixing experiments are usually interpreted in terms of noninteracting two-level systems in order to obtain information on the polarization dephasing time ${\mathit{T}}_2$. Recent experiments involving excitonic resonances in semiconductor quantum wells (including results presented in this paper) show striking qualitative deviations from this simple picture. In particular, an exponential tail is observed at low excitation for negative time delays. At high excitation, the four-wave-mixing signal is found to evolve into two distinct temporal maxima. We demonstrate that the microscopic origin of this time dependence can be understood in terms of coherent exciton-exciton interactions. We show in fact that this behavior is more general and should be seen in numerous dense media where strong nonlinear interactions of polarizations occur. In addition to presenting rigorous numerical results, we analyze two simple situations in which such interactions exist: dielectric media with local-field effects and the anharmonic oscillator. We derive analytical expressions for their time-dependent four-wave-mixing response and discuss the physical origin of these new nonlinear-optical effects.